Electronic Spin Alignment within Homologous NiS2/NiSe2 Heterostructures to Promote Sulfur Redox Kinetics in Lithium‐Sulfur Batteries
Source abstract
Abstract
Abstract The catalytic activation of the Li‐S reaction is fundamental to maximize the capacity and stability of Li‐S batteries (LSBs). Current research on Li‐S catalysts mainly focuses on optimizing the energy levels to promote adsorption and catalytic conversion, while frequently overlooking the electronic spin state influence on charge transfer and orbital interactions. Here, hollow NiS2/NiSe2 heterostructures encapsulated in a nitrogen‐doped carbon matrix (NiS2/NiSe2@NC) are synthesized and used as a catalytic additive in sulfur cathodes. The NiS2/NiSe2 heterostructure promotes the spin splitting of the 3d orbital, driving the Ni3+ transformation from low to high spin. This high spin configuration raises the electronic energy level and activates the electronic state. This accelerates the charge transfer and optimizes the adsorption energy, lowering the reaction energy barrier of the polysulfides conversion. Benefiting from these characteristics, LSBs based on NiS2/NiSe2@NC/S cathodes exhibit high initial capacity (1458 mAh·g⁻1 at 0.1C), excellent rate capability (572 mAh·g⁻1 at 5C), and stable cycling with an average capacity decay rate of only 0.025% per cycle at 1C during 500 cycles. Even at high sulfur loadings (6.2 mg·cm⁻2), high initial capacities of 1173 mAh·g⁻1 (7.27 mAh·cm⁻2) are measured at 0.1C, and 1058 mAh·g⁻1 is retained after 300 cycles.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Catalonia Institute for Energy Research‐IREC Sant Adrià de Besòs Barcelona 08930 Spain
Department of Chemistry University of Barcelona Barcelona 08028 Spain
Catalan Institute of Nanoscience and Nanotechnology (ICN2) CSIC and BIST Campus UAB Bellaterra Barcelona Catalonia 08193 Spain
Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education & School of Physical Science & Technology Lanzhou University Lanzhou 730000 China
School of Chemistry South China Normal University Guangzhou 510006 P. R. China
Analysis and Testing Center South China Normal University Guangzhou 510006 China
Institute for Superconducting and Electronic Materials Australian Institute of Innovative Materials Innovation Campus University of Wollongong Wollongong NSW 2500 Australia
Institute for Advanced Study Chengdu University Chengdu 610106 China
College of Chemistry and Chemical Engineering Chongqing University of Technology Chongqing 400054 China
Institut de Ciència de Materials de Barcelona Campus de la UAB Bellaterra Catalonia 08193 Spain
ICREA Pg. Lluis Companys Barcelona Catalonia 08010 Spain
Funding
European Commission · Natural Science Foundation of Sichuan Province · Ministerio de Ciencia e Innovación
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